Synthesis and characterisation of sesquioxidic precipitates formed by the reaction of acid mine drainage with fly ash leachate

dc.contributor.advisorFey, M. V.
dc.contributor.authorBurgers, C. L. (Colleen Lucie)
dc.contributor.otherUniversity of Stellenbosch. Faculty of Agrisciences. Dept. of Soil Science.
dc.descriptionThesis (MScAgric)--University of Stellenbosch, 2003.en_ZA
dc.description.abstractENGLISH ABSTRACT: Coal mining in South Africa is estimated to produce 200 Ml of acid mine drainage (AMD) per day in the Pretoria-Witwatersrand-Vereeniging (PWV) area alone, while electricity production resulted in approximately 27 Mt of ash in 2001. A large number of collieries in South Africa are tied to power stations where these two waste streams, acid mine drainage and fly ash, have the capacity to neutralize each other and provide an opportunity for co-disposal. The aim of this study was to investigate the reactions that occur during the co-disposal of fly ash leachate (FAL) and AMD and to examine the precipitates that result from the neutralisation reactions. Potentiometric titration was employed to investigate the neutralisation of Al-Fe salt solutions, simulating acid mine drainage (AMD), with alkaline solutions of Ca or Na hydroxide as well as fresh alkaline leachate from fly ash (FAL). The effectiveness of fly ash in removing metals and other salts from acid mine water was examined by analysing the neutralised water and modelling the results thermodynamically. Precipitates, prepared from large scale synthetic AMD and FAL co-disposal at various pH levels and Fe:Al ratios, were characterised according to composition, mineralogy and surface properties. The experimental neutralisation of synthetic acid mine drainage was achieved through titrating the components of SAMD (Fe and Al salt solutions) and solutions of various Fe:Al mole ratios with different bases in air and N2, and comparing the SAMD-FAL system with these simple acids and bases. The FAL used in all experiments was produced from fresh fly ash collected at Arnot power station. The SAMD was prepared as a solution with a pH of 2.5 and containing 12.7 mmol/L Al, 10.9 mmol/L Fe and 40.8 mmol/L SO4. The characterisation of reaction solids was achieved by collecting the precipitates formed from the co-disposal of FAL and SAMD with Fe:Al ratios of 7.3, 0.8 and 2.5. From the titration experiments it was found that upscale potentiometric titrations of SAMD show buffer zones at pH values of 3.5, 4, 6 and 10 corresponding to Fe(III)precipitation, Al precipitation, Fe(II) hydrolysis and oxidation, and Al redissolution, respectively, while downscale potentiometric titrations with SAMD show buffer zones at pH values 12 – 11, 9 and 4.5, which correspond to Fe oxidation and precipitation, Al precipitation and Al re-dissolution, respectively. A high concentration of Al in the simulated AMD inhibited the crystallinity of the precipitates and resulted in a large quantity of SO4 being removed from solution, which suggests that an aluminium sulphate phase is precipitating, but it is not crystalline and cannot be identified by XRD. Titrations performed up-scale by adding FAL to AMD showed near-complete metal and substantial SO4 removal from solution. The characterisation of reaction solids by x-ray diffraction, infrared spectroscopy, thermal gravimetric and differential thermal analysis revealed that the precipitates consist of poorly crystalline, highly Al-substituted goethite and ferrihydrite with large amounts of SO4 included in the structure. Poorly crystalline bayerite appears at a high pH and high Al concentration, and calcite is present in precipitates made by adding SAMD to FAL. High surface charges of between 330 cmolc/kg positive and 550 cmolc/kg negative charge and potentially large specific surface areas between 7 and 236 m2/g suggest a strong potential for the precipitates to function as low-grade adsorbents in wastewater treatment. The similarity of these ochre precipitates to soil minerals implies that land disposal of the neutralised solids is also viable.en_ZA
dc.description.abstractAFRIKAANSE OPSOMMING: Steenkool mynbou in SA produseer na benaming 200 ML suur mynwater per dag in die PWV area alleenlik, terwyl opwekking van elektrisiteit naastenby 27 Mt vliegas geproduseer het in 2001. ’n Groot aantal steenkoolmyne in SA word verbind met kragsentrales, waar hierdie twee strome afval, suur mynwater en vliegas, die kapasiteit het om mekaar te neutraliseer en die weg te baan vir gesamentlike wegdoening. Die doel van hierdie studie was om die reaksies wat plaasvind gedurende gesamentlike wegdoening van vliegas loog (VAL) en suur mynwater (SMW) te ondersoek, asook die neerslae wat mag vorm as gevolg van neutralisasie reaksies. Potensiometriese titrasies was gebruik om die neutralisering tussen Al:Fe-sout oplossings te ondersoek as nabootsing van SMW met gebruikmaking van alkaliese oplossings van Ca of Na hidroksied asook vars loog van VA. Die effektiwiteit van VA om metale en soute uit SMW te verwyder was getoets deur outleding van die geneutraliseerde water en modellering van die termodinamika. Neerslae berei uit groot-skaal sintetiese SMW en VAL en met gelyktydige storting by verskeie pH vlakke en Fe:Al verhoudings, was gekarakteriseer volgens samestelling, mineralogie en oppervlak eienskappe. Die eksperimentele neutralisering van sintetiese suur mynwater (SSMW) was gedoen deur titrering van die SSMW komponente en oplossings van verskeie Fe:Al molêre verhoudings met verskillende basisse in lug en N2, en vergelyking van SSMW-VAL sisteem met hierdie eenvoudige sure en basisse. Die VAL gebruik in alle eksperimente was geproduseer van vliegas verkry van die Arnot kragsentrale. Die SSMW was berei as ’n oplossing met ’n pH van 2.5 en bevat 12.7 mmol/L Al, 10.9 mmol/L Fe en 40.8 mmol/L SO4. Die karakterisering van vastestowwe uit die reaksie was gedoen deur die bemonstering van neerslae gevorm as gevolg van die gelyktydige wegdoening van VAL en SSMW met Al:Fe verhoudings van 7.3, 0.8 en 2.5.Die was waargeneem in die titrasie eksperimente dat hoër-skaal potensiometriese titrasie van SSMW buffersones, by pH waardes 3.5, 4, 6 en 10, ooreenstem met Fe(III) presipitasie, Al presipitasie, Fe(II) hidrolise en oksidasie, en Al her oplossing, terwyl laer skaal potensiometriese titrasie met SSMW buffer sones by pH waardes 12 - 11, 9 en 4.5 ooreenstem met Fe(III) presipitasie en oksidasie, Al presipitasie en heroplossing respektiewelik. ’n Hoë konsentrasie Al in die sintetiese SMW het kristalliniteit van die neerslae geïnhibeer en veroorsaak dat ’n hoeveelheid SO4 uit oplossing verwyder is, wat suggereer dat die AlSO4 fase neerslaan maar nie kristallyn is en gevolglik nie opgetel word met x-straal diffraksie nie. Titrasies gedoen by hoërskaal deur byvoeging van VAL tot SSMW, het feitlik volledige metaal en SO4 verwydering uit oplossing getoon. Die karakterisering deur x-straal diffraksie, infrarooispektroskopie, termies gravimetries en differentiële termiese analise, het getoon dat die presipitate bestaan uit swak kristallyne, hoë Al-gesubstitueerde goethiet en ferrihidriet met groot hoeveelhede SO4 vasgevang in die struktuur. Swak kristallyne bayeriet verskyn by hoë pH en hoë Al-konsentrasies en kalsiet is teenwoordig in neerslae gevorm deur byvoeging van SSMW tot VAL. Hoë oppervlakladings van tussen 330 cmolc/kg positief en 550 cmolc/kg negatiewe lading en ook potensieel groot spesifieke oppervlak van tussen 7 en 236 m2/g, dui op ’n sterk potensiaal vir neerslae om as laegraadse adsorbeermiddels in afvalwaterbehandeling gebruik te word. Die ooreenstemming in hierdie geelbruin neerslae met grond minerale, impliseer dat die land storting van geneutraliseerde vastestowwe ook lewensvatbaar
dc.format.extentxiv, 110 leaves : ill.
dc.publisherStellenbosch : University of Stellenbosch
dc.subjectAcid mine drainageen_ZA
dc.subjectFly ashen_ZA
dc.subjectSewage sludge precipitantsen_ZA
dc.subjectTheses -- Agricultureen_ZA
dc.subjectDissertations -- Agricultureen_ZA
dc.subjectTheses -- Soil scienceen
dc.subjectDissertations -- Soil scienceen
dc.titleSynthesis and characterisation of sesquioxidic precipitates formed by the reaction of acid mine drainage with fly ash leachateen_ZA
dc.rights.holderUniversity of Stellenbosch

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